Electrical conduction through bond percolation in Nd0.67Sr0.33MnO3

We report our analysis of resistivity data on Nd_0.67Sr_0.33MnO₃ polycrystalline samples as a function of preparative conditions using a bond percolation model for a random mixture of metallic and insulating regions, assuming polaronic transport above and below the metal-insulator (M-I) transition temperature. Our analysis suggests that for oxygen deficient compounds the M-I transition that occurs at a lower temperature than the ferromagnetic transition arises from a percolation of the metallic regions. The temperature dependence of resistivity and thermopower suggests the existence of a bimodal distribution of conductivities.     

Vibrational anisotropy of MnO6 octahedron and phase separation in La0.67−yPryCa0.33MnO3 manganites

The role of vibrational anisotropy of Mn³⁺O₆ octahedron in the phase separation behavior of La_0.67−yPr_yCa_0.33MnO₃ (x=0, 0.15, 0.25 and 0.30) has been investigated by means of magnetization M, internal friction Q⁻¹, Young's modulus E along with the X-ray powder diffraction measurements. For the samples with y=0 and 0.15, the Q⁻¹ exhibits three peaks in the ferromagnetic region, which are attributed to the intrinsic inhomogeneity of ferromagnetic phase, i.e. the electronic phase separation with the coexistence of insulating and conducting phases. However, both the samples with y=0.25 and 0.30 undergo a magnetic phase separation with the coexistence of the antiferromagnetic and ferromagnetic phases, and the Q⁻¹ peaks related to the electronic phase separation have not been observed. In addition, the Q⁻¹ exhibits a peak in the paramagnetic region for all samples, which may result from the formation of magnetic clusters. We observed that the evolution from electronic to magnetic phase separation is close related to the rapid increase in the ratio of two kinds of Jahn-Teller distortion modes Q₃ and Q₂, i.e. Q₃/Q₂. A schematic phase diagram is given in the text, and it is suggested that the enhancement of vibrational anisotropy of Mn³⁺O₆ octahedron plays a key role in the evolution from electronic to magnetic phase separation.     

Magnetic and electrical behavior of La1−xAxMnO3 (A=Li, Na, K and Rb) manganites

With a view to understand the magnetic and electrical behavior of monovalent substituted lanthanum manganites, a series of materials were prepared by sol-gel route by sintering at 1200 °C. The X-ray diffraction data were analyzed using Rietveld refinement technique and it has been found that all the samples were found to crystallize into rhombohedral structure with R3¯c space group. The values of ferro to paramagnetic (T_C) and metal-insulator transition (T_P) temperatures were obtained using ac susceptibility and electrical resistivity data, respectively. It has been found that sodium-, potassium- and rubidium-doped samples exhibit two peaks in the electrical resistivity vs. temperature plots. The observed behavior has been explained on the basis of oxygen deficiency present in the samples. The electrical resistivity data were analyzed using various theoretical models and it has been concluded that the electrical resistivity data in the low-temperature regime (T<T_P) can be explained using the equation ρ_(T)=ρ₀+ρ₂T²+ρ_4.5T^4.5, signifying the importance of the grain/domain boundary, electron-electron and two magnon scattering processes. On the other hand, the high-temperature resisitivity data (T>T_P) were explained using variable range and small polaron hopping mechanisms.     

On the coexistence of spin and lattice polarons in the La0.67−xEuxCa0.33MnO3 CMR system

The electrical and magnetic transport properties of the La_0.67−xEu_xCa_0.33MnO₃ system exhibit lowering of insulator to metal and paramagnetic to ferromagnetic transition temperature (T_C) with the increase of Eu concentration in addition to possessing CMR property. The temperature variation of electrical resistivity and magnetic susceptibility for x=0.21 is found to have two distinct regions in the paramagnetic state for T>T_P; one with the localization of lattice polaron in the high-temperature region (T>1.5T_P) satisfying the dynamics of variable range hopping (VRH) model and the other being the combination of the spin and lattice polarons in the region T_P<T<1.5T_P. The resistivity variation with temperature and magnetic field, the cusp in the resistivity peak and CMR phenomenon are interpreted in terms of coexistence of spin and lattice small polarons in the intermediate region (T_P<T<1.5T_P). The spin polaron energy in the La_0.46Eu_0.21Ca_0.33MnO₃ system is estimated to be 106.73±0.90 meV and this energy decreases with the increase of external magnetic field. The MR ratio is maximal with a value of 99.99% around the transition temperature and this maximum persists till T→0 K, at the field of 8 T.     

Electric current-induced giant electroresistance in epitaxial La0.67Sr0.33MnO3 thin films

The electronic transport behavior of La_0.67Sr_0.33MnO₃ epitaxial thin films with different thicknesses has been investigated under various applied DC currents. The 20 and 70 nm thick films show a giant negative electroresistance (ER). In contrast, the films with 100 nm thickness show unusual giant positive ER, which can reach 30% with the current density of 1.8×10⁸ A/cm² at room temperature. It is interesting that the electric current can also change the magnetoresistance of the films. The results were explained by considering the spin polarized current induced increase of ferromagnetic metallic phase and current-induced lattice distortion via electron wind force under high current density.     

Superparamagnetic behavior of La0.67Sr0.33MnO3 nanoparticles prepared via sol-gel method

Magnetic nanoparticles of La_0.67Sr_0.33MnO₃ (LSMO) manganite were prepared by sol-gel method. Phase formation and crystal structure of the synthesized powder were examined by the X-ray diffraction (XRD) using the Rietveld analysis. The mean particle size was determined by the transmission electron microscopy (TEM). Infrared transmission spectroscopy revealed that stretching and bending modes are influenced by calcinations temperature. The temperature dependence of the ac magnetic susceptibility was measured at different frequencies and ac magnetic fields in the selected ranges of 40-1000 Hz and 80-800 A/m, respectively. The temperature dependence of ac susceptibility shows a characteristic maxima corresponding to the blocking temperature near room temperature. The frequency dependence of the blocking temperature is well described by the Vogel-Fulcher law. By fitting the experimental data with this law, the relaxation time τ₀=1.7×10⁻¹² s, characteristic temperature T₀=262±3 K, anisotropy energy E_a/k=684±15 K and effective magnetic anisotropy constant k_eff=2.25×10⁴ erg/cm³ have been obtained. dc Magnetization measurement versus magnetic field shows that some of LSMO nanoparticles are blocked at 293 K. The role of magnetic interparticle interactions on the magnetic behavior is also investigated.     

Evidence for instability in charge ordering Nd0.5Sr0.5MnO3

The transport properties and magnetic phase transitions of charge ordering manganites Nd_0.5Sr_0.5MnO₃ have been investigated. From resistivity measurements, a continuous increase of resistivity upon the thermal cycling occurs at , and shows an instable behavior in the system. The experimental results of magnetization and electron-spin-resonance spectra indicate that the ferromagnetic phase and antiferromagnetic phase coexist in a broad temperature region. We think that the origin of the instability stems from an inhomogeneous strain yielded in the ferromagnetic interface, due to the competition among different phases.     

Magnetotransport properties of La0.67Ca0.33MnO3//La0.67Sr0.33MnO3 bilayers

The perovskite bilayers La0.67Ca0.33MnO3 （LCMO） （100 nm） / La0.67Sr0.33MnO3（LSMO） （100 nm） and LSMO （100 nm） / LCMO （100 nm） are fabricated by a facing-target sputtering technique. Their transport and magnetic properties are investigated. It is found that the transport properties between them are different obviously due to distinguishable structures, and the different lattice strains in both films result in the difference of metal-to-insulator transition. Only single-step magnetization loop appears in our bilayers from 5K to 320K, and the coercive force of LSMO/LCMO varies irregularly with a minimum ～ 2387A/m which is lower than that of LCMO and LSMO single layer films. The behaviour is explained by some magnetic coupling.     

Highly cation-deficient manganese perovskite, La1−xMn1−yO3 with x=y

Oxidative (δ>0) nonstoichiometry in the perovskite ‘LaMnO_3+δ’ has been known to be manifested not with O interstitials but rather with cation vacancies of equal amounts at the two cation sites, La and Mn, i.e. La_1−xMn_1−yO₃ with x=y. Here, we report the fabrication of samples with record-high cation-vacancy concentrations (x>0.12 or δ>0.4) by means of a variety of high-pressure oxygenation techniques. Linear (negative) dependence of the cell volume on x was observed within the whole x range investigated, down to 56.9 Å³ (per formula unit) for a sample oxygenated at 5 GPa and 1100 °C using Ag₂O₂ as an excess oxygen source. With increasing degree of cation deficiency in La_1−xMn_1−xO₃, the ferromagnetic transition temperature was found to follow a bell shape with respect to x exhibiting a maximum of ∼250 K about x≈0.1. For moderately oxygenated samples large magnetoresistance effect was evidenced.     

Elastic anomalies of La0.67Sr0.33−xBaxMnO3 in the vicinity of TC

With a view to understand the elastic behaviour of a material system, La_0.67Sr_0.33−xBa_xMnO₃ (where x=0, 0.1, 0.2, and 0.33) especially in the vicinity of their magnetic transition temperature T_C, a systematic investigation of ultrasonic velocity over a temperature range 300-400 K has been carried out. The materials prepared by citrate gel route, were characterized structurally by XRD and on analyzing the XRD patterns, it has been concluded that all the samples are having rhombohedral structure with space group of R3?c. The magnetic (T_C) transition temperatures determined by AC susceptibility measurements are found to decrease continuously with increasing barium concentration. Finally, the ultrasonic longitudinal velocities of all the samples are found to exhibit considerable softening in the vicinity of their magnetic transition temperatures, T_C and the observed behaviour is explained using mean field theory and Jahn-Teller theorem.     

Magnetoresistance and electron paramagnetic resonance study of La0.67−yYyBa0.33MnO3/LaAlO3 thin films

Magnetoresistive La_0.67−yY_yBa_0.33MnO₃/LaAlO₃ thin films were prepared by the sol-gel spin-coating method. Our resistivity and the electron spin resonance (ESR) measurements indicate that the main factor determining the metal-insulator transition temperature T_m is the cation disorder represented by the cation radii variance σ², and that ferromagnetic insulating regions coexist in the ferromagnetic metallic phase. In the paramagnetic phase, the dissociation energy of spin clusters and the polaron hopping energy obtained from the ESR intensity and linewidth also displayed a prominent dependence on σ². Polaron localization due to Jahn-Teller distortions appears to be responsible simultaneously for the decrease in the ferromagnetic order and for the increase in the orbital order.     

Jahn-Teller transition and electron-phonon interaction in Cr-doped manganites Sr0.9Ce0.1Mn1−yCryO3

Cr-doped manganites Sr_0.9Ce_0.1Mn_1−yCr_yO₃ (y=0, 0.05, and 0.10) have been systematically investigated by X-ray, magnetic, transport, and elastic properties measurements. For parent compound Sr_0.9Ce_0.1MnO₃, it undergoes a metal-insulator (M-I) transition at 318 K, which is suggested to originate from a first-order structural transition accompanied by Jahn-Teller (JT) transition. With increasing Cr doping content, the JT transition temperature decreases. The Cr doping suppresses the antiferromagnetic (AFM) state and makes the system spin-glass (SG) behavior at low temperatures. In the vicinity of JT transition temperatures, the softening of Young's modulus originating from the coupling of the orbital (quadrupolar) moment of the e_g orbital of Mn³⁺ ion to the elastic strain has been observed. The anomalous Young's modulus properties imply the electron-phonon coupling due to the JT effect may play an important role in the system.     

Structural, magnetic and transport properties in the manganites La0.7Sr0.3−xTexMnO3 (0≤x≤0.15)

The effect of Te-doping at La-site on structural, magnetic and transport properties in the manganites La_0.7Sr_0.3−xTe_xMnO₃ (0≤x≤0.15) has been investigated. All samples show a rhombohedral structure with the space group . It shows that the Mn-O-Mn bond angle decreases and the Mn-O bond length increases with the increase of Te content. The Curie temperature T_C decreases with increasing Te-doping level, in contrast, the magnetization magnitude of Te-doping samples at low temperatures increase with increasing x as x≤0.05 and then decrease with further increasing x to 0.15. The results are discussed in terms of the combined effects of the opening of the new double exchange (DE) channel between Mn²⁺-O-Mn³⁺ due to the introduction of Mn²⁺ ions because of the substitution of Te⁴⁺ for Sr²⁺ and the reduction of the transfer integral b due to the decrease of the Mn-O-Mn bond angle.     

Room temperature magnetoresistance in Ln2/3A1/3MnO3 manganites

The investigation of the manganites La_2/3−xPr_xSr_1/3MnO₃, La_2/3Sr_1/3−xCa_xMnO₃ and La_2/3+xCa_1/3−2xAg_xMnO₃, which all exhibit Mn³⁺:Mn⁴⁺=2, shows that it is possible to reach high magnetoresistance at room temperature, up to 21% under 1.2 T. These materials are compared to La_5/6Ag_1/6MnO₃ which corresponds to the same Mn³⁺:Mn⁴⁺ ratio and exhibits a magnetoresistance of 25% in this field. An interesting feature deals with the value of the insulator-metal transition temperature T_IM, often higher than T_C, especially for Ag-based compounds. It is suggested that the latter results either from a better oxygenation of the surface of the grains or from a migration of silver toward the surface.     

Heat capacity and magnetocaloric effect in manganites (La1−yEuy)0.7Pb0.3MnO3 (y:0.2; 0.6)

Heat capacity and intensive magnetocaloric effect (MCE) in manganites (La_1−yEu_y)_0.7Pb_0.3MnO₃ [y=0.2; 0.6] (LEPM) were investigated by means of adiabatic calorimeter. The heat capacity anomaly as well as the values of both the intensive (ΔT_AD) and the extensive (ΔS_MCE) MCE were found to decrease upon increased replacement of La with nonmagnetic Eu. However, because of widening of the MCE peaks, the LEPM compounds show the relative cooling power, RCP/ΔH, comparable to other solid solutions of manganites. Owing to strong effect of Eu→La substitution on the Curie temperature, LEPM might have potential as the solid state refrigerants in multi-element cooling apparatus operating in a wide temperature range.     

Magnetoresistance in La1−xCaxMnO3 (0≤x<0.4)

The magnetic and transport properties of La_1−xCa_xMnO₃ (0≤x<0.4) have been systematically studied. The magnetoresistance (MR) maximum appears at x=0.2-0.25 and the temperature dependence of MR for x>0.25 shows a much broader profile than that of samples for x=0.2-0.25. Based on a scenario in which there is a short-range charge ordering (CO) state coexisting in the ferromagnetic state matrix for x>0.25, and the least or even no short-range CO state exists in samples for x=0.2-0.25, the above observations can be understood.     

Thickness dependence of electroresistance in La0.67Ca0.33MnO3 epitaxial films

The electroresistance (ER) of La_0.67Ca_0.33MnO₃ (LCMO) epitaxial thin films with different thicknesses was studied. For the 110 nm thick LCMO film, its ER shows a maximum at T_p, where the resistance shows a peak, and decreases to zero at lower temperatures. While for the 30 nm thick LCMO film, its ER is remarkable in a wide temperature range. Another interesting observation in this work is that the electric current can tune the magnetoresistance of the ultrathin LCMO thin film. The results were discussed by considering the coexistence of ferromagnetic metallic phase with the charge ordered phase, and the variation of the phase separation with film thickness and electric current. This work also demonstrates that electric current can tune the magnetoresistance of the manganites, which is helpful for their applications.     

Correlation between extrinsic magnetoresistance and electroresistance in La0.6Pb0.4MnO3 thin films as revealed from current-voltage and ferromagnetic resonance studies

We have investigated magnetoresistance (MR) and electroresistance (ER) of well characterized La_0.6Pb_0.4MnO₃ (LPMO) films having two different crystallinity (i) (00l) oriented single-crystalline, SC, i.e. without any grain boundaries, and (ii) nanocrystalline, NC, with an average grain size of 17 nm. Both MR and ER were remarkably different for the two films, that is, (i) NC films exhibited a highest MR of ∼100% near the metal-insulator transition temperature; while for SC films the MR was in the range of 40-60%, (ii) NC films exhibited a finite ER, which increased monotonically with decreasing temperature; while in SC films ER was completely absent. Using current-voltage characteristic and ferromagnetic resonance studies we demonstrate that both enhanced MR and ER in NC films are extrinsic in nature and originate due to the presence of spin glassy grain boundaries.     

Structure and magnetization studies of Nd0.5−xPrxSr0.5MnO3 system

The structural and magnetic properties of Nd_0.5−xPr_xSr_0.5MnO₃ (x=0, 0.1, 0.2, 0.3, 0.4 and 0.5) system have been investigated. With the substitution of Pr in Nd_0.5Sr_0.5MnO₃, it shows a gradual structure transformation from the Imma orthorhombic symmetry to the tetragonal I4/mcm phase, and the crystallographic transition remains incomplete, even in Pr_0.5Sr_0.5MnO₃. A large bifurcation between zero-field-cooled (ZFC) and field-cooled (FC) susceptibility has been observed below Curie temperature (T_C), which is characteristic of coexistence of ferromagnetism (FM) and antiferromagnetism (AFM) at low temperature region. The magnetization of Pr_0.5Sr_0.5MnO₃ is larger than that of Nd_0.5Sr_0.5MnO₃, while Nd_0.5Sr_0.5MnO₃ with more CE-type AFM shows larger magnetization than Nd_0.3Pr_0.2Sr_0.5MnO_3, which mixed with CE-type (majority) and A-type (minority) AFM at low temperature, indicating that the magnetization of Nd_0.5−xPr_xSr_0.5MnO₃ system is affected by A-site disorder combined with orbital ordering of A-type AFM and CE-type AFM.     

Large room-temperature magnetoresistance and temperature-dependent magnetoresistance inversion in La0.67Sr0.33MnO3/Alq3 - Co nanocomposites/Co devices

Large room-temperature (RT) magnetoresistance (MR) and temperature-dependent MR inversion have been observed in tris (8-hydroxyquinoline) aluminum (Alq₃)-cobalt nanocomposites-based organic-inorganic hybrid devices. Negative MR-high resistance for parallel electrodes configuration — due to magnetization reversal of ferromagnetic (FM) electrodes has been observed at low temperatures. As the temperature increases, the MR undergoes a sign change. At room temperature, a positive MR of ∼9.7% with the resistivity dropping monotonously with increasing magnetic fields has been observed. The RT MR is about two orders of magnitude of that in organic-FM nanocomposites measured with nonmagnetic electrodes. The enhancement of RT MR is attributed to the injection of spin polarized carriers into Alq₃-Co nanocomposites.